In this paper, we focus on left-invariant m-quasi-Einstein metrics on simple Lie groups. First, we prove that X is a left-invariant Killing vector field if the metric on a compact simple Lie group is m-quasi-Einstein. Then we show that every compact simple Lie group admits non-trivial m-quasi-Einstein metrics except SU (3), E 8 and G 2 and most of them admit infinitely many metrics. Moreover, we prove that every compact simple Lie group admits non-trivial m-quasi-Einstein Lorentzian metrics and most of them admit infinitely many metrics. Finally, we prove that some non-compact simple Lie groups admit infinitely many non-trivial m-quasi-Einstein Lorentzian metrics.